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Enhanced energy transfer and conversion for high performance phononic crystal-
assisted elastic wave energy harvesting

Tae-Gon Lee, Soo-Ho Jo, Hong Min Seung, Sun-Woo Kim, Eun-Ji Kim, Byeng D.
Youn, Sahn Nahm, Miso Kim
PII: S2211-2855(20)30804-1
DOI: https://doi.org/10.1016/j.nanoen.2020.105226
Reference: NANOEN 105226

To appear in: Nano Energy

Received Date: 23 May 2020


Revised Date: 13 July 2020
Accepted Date: 23 July 2020

Please cite this article as: T.-G. Lee, S.-H. Jo, H.M. Seung, S.-W. Kim, E.-J. Kim, B.D. Youn, S. Nahm,
M. Kim, Enhanced energy transfer and conversion for high performance phononic crystal-assisted
elastic wave energy harvesting, Nano Energy (2020), doi: https://doi.org/10.1016/j.nanoen.2020.105226.

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Graphical Abstract

Metamaterials such as phononic crystals and acoustic/elastic metamaterials provide an ideal

platform to manipulate mechanical waves and enable amplification of input mechanical wave

energy, such as sound, vibration, and ultrasonic waves, thus enabling drastic enhancement of

energy harvesting. In this study, a rational parametric design strategy is established to produce a

proper piezoelectric ceramic device that can substantially enhance the phononic crystal-assisted

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elastic wave energy harvesting performance.

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KEYWORDS Metamaterials, Phononic crystals, Energy harvesting, Piezoelectricity, Elastic

waves
Enhanced Energy Transfer and Conversion for High Performance

Phononic Crystal-Assisted Elastic Wave Energy Harvesting

Tae-Gon Leea, Soo-Ho Job, Hong Min Seungc, Sun-Woo Kimd, Eun-Ji Kimd, Byeng D. Younb,

Sahn Nahma,d*, and Miso Kimc*

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a
Department of Nano Bio Information Technology, KU-KIST Graduate School of Converging

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Science and Technology, Korea University, Seoul, 02841, Republic of Korea
b
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Department of Mechanical and Aerospace Engineering, Seoul National University, Seoul 08826,
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Republic of Korea
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c
Korea Research Institute of Standards and Science (KRISS), Daejeon 34113, Republic of Korea
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d
Department of Materials Science and Engineering, Korea University, Seoul, 02841, Republic of

Korea
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*Correspondence to: Sahn Nahm (snahm@korea.ac.kr) and Miso Kim (misokim@kriss.re.kr)


Abstract

A critical challenge in energy harvesting has been insufficient sustainable power generation for

practical applications, despite the benefits of self-powering and green-enabling technology.

Metamaterials are artificial structures capable of controlling and manipulating functionalities

beyond the limit of natural materials. Various metamaterial concepts including phononic crystals

(PnCs) and locally resonant metamaterials have proved to manipulate mechanical waves and

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enable amplification of input mechanical wave energy, such as sound, vibration, and ultrasonic

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waves, thus enabling drastic enhancement of energy harvesting thus far. Along with the need for

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research on novel metamaterial designs for energy localization and focusing, fundamental
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understanding of the energy transfer and conversion at the interface between the piezoelectric
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energy harvesting (PEH) devices and the metamaterial host structure is also crucial to further

enhancing the output power performance of metamaterial-based energy harvesting. Here, we


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report a substantially enhanced harvesting power amplification and output power in phononic
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crystal-assisted elastic wave energy harvesting by tailoring geometric and materials parameters
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of a PEH device for a given PnC structure. We envision that the underlying wave physics and

materials science in this rational parametric design strategy will contribute to realizing self-

powered sensor applications in industrial and environmental monitoring fields.

Keywords: Metamaterials, Phononic crystals, Energy harvesting, Piezoelectricity, Elastic waves


1. Introduction

Beyond the development of high-performance energy harvesting materials, devices, and

circuits [1-6], the ability of metamaterials to actively manipulate and deliver input mechanical

waves toward a desired location provides a new approach to unlock drastic improvements in the

energy harvesting performance. Metamaterials are artificially engineered structures that can

exhibit nonconventional and unique effective material properties and phenomena, such as

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negative refractive index [7,8] and band gaps [9,10]. These properties enable wave manipulation

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not only in photonic [11,12], but also in mechanical regimes, where acoustic, vibration, and

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elastic waves are involved [13–15], offering potential application opportunities for vibration and
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sound control [16,17], acoustic and elastic superlenses [18-20], and importantly energy focusing
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and harvesting [21,22]. Metamaterial-based energy harvesting (MEH) is a new paradigm of

energy harvesting systems, which pushes the boundaries to drastic harvesting performance
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enhancement through tailoring and amplification of input mechanical wave energy. Various
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intriguing metamaterial concepts, including phononic crystals [23,24], gradient index (GRIN)
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phononic crystals [25,26], acoustic black holes [27,28], and locally resonant acoustic

metamaterials [29,30] have actively been explored for energy focusing and harvesting purposes.

As in the early stage of research, the analysis and fabrication of new or existing concepts of

metamaterial designs and their simple integration with energy harvesting devices have been the

sole focus in MEH research thus far. Indeed, more novel metamaterial designs are still required

for further improvement in energy focusing performance with both direction and magnitude

controllability as well as for size reduction and broadband frequency operation. Along with the

development of new metamaterial designs, the fundamental understanding of the underlying

energy transfer and conversion mechanisms that occur particularly at the interface between the
piezoelectric energy harvesting device integrated into the metamaterial platform and the host

structure of metamaterial is also crucial for further improvement in MEH output performance.

However, the detailed relationship between the physical properties of energy harvesting devices

and the metamaterial has not been elucidated to date.

In this study, we aim to realize a high performance MEH system by identifying proper

geometric and material properties of a piezoelectric ceramics disk as an energy harvesting (EH)

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device for a given PnC platform. Phononic crystals that consist of a periodic arrangement of unit

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cells belong to the class of metamaterials [31]. The interaction of elastic waves with unit cells in

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a PnC creates a band gap, within which further propagation of waves is prohibited. Evanescent
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waves scattered from the unit cells in a PnC are trapped within this band gap regime, and thus so
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is the elastic energy. The confined energy can be localized at the defect created inside the PnC,

where periodicity is broken by introducing a foreign element or eliminating an existing unit cell.
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Once amplification of input elastic wave energy occurs through wave manipulation at the defect
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inside the phononic crystal (PnC) [23,24], the overall harvesting power performance of MEH
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depends on how efficiently this amplified energy is transferred to the harvesting device with

minimal loss through the interface. Energy amplification is determined by the wave control

characteristic of the metamaterial itself, which in this case is the PnC; efficient energy transfer

and absorption, is related to the understanding of wave dynamics through the interface between

the PnC and piezoelectric energy harvester (PEH). We identified proper geometric parameters for

a PEH that enables highly efficient energy transfer from the host medium structure PnC to the

EH device considering the mechanical impedance matching between the PEH and PnC, as well

as the voltage cancellation effect due to wave behavior inside the PnC. The transferred energy is

then converted into electrical energy through the piezoelectric effect, where a selection of high-
performance piezoelectric material with large figure-of-merit d × g values should be employed.

Enhanced energy transfer and conversion through a PEH device via parametric studies yields

substantial improvement of PnC-based EH performance up to 2.7 mW, the largest output power

ever reported in elastic wave energy harvesting.

2. Results and Discussion

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2.1 Phononic crystal-assisted elastic wave energy localization and harvesting

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We proposed a design of two-dimensional phononic crystals consisting of octagonal hole-

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type unit cells through geometric and band gap optimization process and confirmed energy
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confinement and drastic enhanced energy harvesting at the defect of the proposed PnCs at the
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target frequency of 50 kHz both analytically and experimentally in our previous work [23]. The

same two-dimensional octagonal hole-type PnC design is adopted here as a metamaterial


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platform except that the supercell size is extended to 5 × 11 (Fig. 1(a)) of a 2-mm thick
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aluminum plate, instead of the 5 × 7 supercell used in prior work for further energy confinement.
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A single defect is created by removing one unit cell in the center of the second layer of the

supercell along the direction of incident wave propagation. As fully addressed in our study in

[32], this defect location allows the highest elastic wave localization with less attenuation

through wave propagation to take place, since it is the closest location from the incident waves

moving toward the PnC, while ensuring the periodicity for band gap formation (Fig. 1(a)). The

band structures and the energy localization performance at the defect of the octagonal and

circular hole-type unit cells are fully compared and addressed in the Supplementary S2.

Fig. 1(b) shows the calculated dispersion curve of the PnC 5 x 11 supercell with a defect,

obtained by the finite element method, where the formation of a complete band gap from 46.93
kHz to 52.68 kHz, within which elastic waves originating from any direction would be confined

inside the PnC, is clearly confirmed. Formation of seven defect bands inside the phononic band

gap is also observed as a result of interaction between the defect and the supercell. Fig. 1(c)

demonstrates the simulation result of harmonic wave propagation analysis using the

commercially-available software, COMSOL MULTIPHYSICS version 5.3, where the highest

amplitude at the center of the defect confirms the highest energy localization at this location.

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Upon the incident waves being applied from the left, little propagation is shown to take place

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after the PnC supercell structures, since 50 kHz falls within the bang gap regime. The

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dependence of incident wave directions on energy localization inside the defect of the octagonal
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PnCs is further studied through time harmonic analysis and fully addressed in the Supplementary
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S3. Experimental visualization of wave propagation inside the defect of our PnC supercell is also

successfully presented in Fig. 1(d) from a top-view, where prominent energy localization clearly
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occurs at the center. Inside the defect, elastic waves oscillate with time in the out-of-plane
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direction, while having the maximum amplitude at the defect center, hence revealing the
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monopole defect mode [23] at this frequency. More detailed displacement fields with respect to

time and position are also illustrated in Fig. S7, and the videos showing the displacement fields

are also available in the Supplementary Data. The prominent difference of the mechanical

displacement measured at the center of the defect within the PnC (52 nm) and at the same

location in a bare aluminum plate without the PnC (24 nm) reveals a considerable amplification

effect due to the band gap characteristic of the PnC and the energy localization at its defect (Fig.

1(e)).

We conducted harvesting performance characterization by placing a piezoelectric ceramic

disk at the center of the defect, as illustrated in Fig. 1(a–iv), and measuring the output voltage
and power as functions of time and electrical load resistances. The results of the output voltage

and power in the time domain at various load resistances plotted in Fig. 1(f) and 1(g) correspond

to the case where the diameter and the thickness of the piezoelectric ceramic are 8 mm and 2.0

mm, respectively, and its composition is 0.32PZ-0.39PT-0.29PNN (specimen #2 in Table 1) [33].

The voltage and power exhibit an increasing trend with time and reach their maximum values

after approximately 0.9 ms, following which they exhibit a decreasing trend with oscillating

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behavior for all electrical resistances. The maximum voltage increases with increasing electrical

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resistances and approaches its open-circuit voltage, which is 5.2 V in this case, as shown in Fig.

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1(f). In terms of output power, the maximum value of 2.7 mW appears at its optimal electrical
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resistance of 4.8 kΩ, as shown in Fig. 1(g). The existence of an optimal power value with respect
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to electrical load resistances is a well-known phenomenon in piezoelectric vibration energy

harvesting [34,35], and here we can confirm that the same principle can be applied to elastic
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wave energy harvesting, especially with a PnC. Although the magnitudes of voltage and power
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vary while we vary the geometric and material properties of the piezoelectric ceramic disk
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through this study, the trends in voltage and power as functions of time and load resistances

follow the same trend in those shown in Fig. 1(f) and 1(g), regardless of the parameter variation.

2.2 Enhanced energy transfer via tailoring geometric parameters of a PEH

Efficient energy transfer of the localized elastic energy from the given medium structure PnC

into the PEH device is possible by tuning the geometric dimensions of a PEH. The geometric

variables considered in this work are the diameter and thickness of the PEH consisting of

piezoelectric ceramic disk sandwiched by top and bottom electrodes (Fig. 1(a–iv)). The diameter

represents the degree of PEH coverage area for the given PnC supercell. Although a larger
piezoelectric area might intuitively seem advantageous for more power generation, it has been

uncovered that the strain nodes of vibration modes can cause cancellation of electrical outputs in

harvesting. As a solution to avoiding such cancellation at the nodes, several approaches, such as

multimodal electrode configurations and segmented EH skin concepts, have been proposed in

previous studies [36,37]. Thus, it is essential to assess the proper width required to avoid voltage

cancellation due to the wave dynamics in the PnC and thus maximize electrical output

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performance. Considering that the size of the unit cell is 34 mm, we fabricated PEH disks of 6, 8,

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10, 12, 18, 24, and 36 mm diameter with the thickness and composition of 1.5 mm and 0.23PZ-

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0.36PT-0.41PNN (specimen #1 in Table 1) [38], respectively.
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Fig. 2(a) presents the voltage plots as a function of load resistances for the PEH with various
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diameters. Here, each voltage is taken from the maximum values in the voltage-time plots (Fig.

S8) that are similar to Fig. 1(f). As the diameter increases from 6 mm to 36 mm, the maximum
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voltage (i.e., open-circuit voltage) values are observed to decrease from 3.5 V to 0.1 V. The
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observation of higher voltage generation with smaller diameter is directly related to the wave
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dynamics that occur inside the PnC. The calculated wavelength, λ, of the incident plane waves

generated at 50 kHz in a 2-mm thick aluminum plate is 19 mm, as experimentally confirmed and

illustrated in Fig. 2(d). When these plane waves propagate and enter the defect of the PnC

supercell, the resulting monopole defect mode experimentally observed in Fig. 1(d) forces the

medium aluminum plate to oscillate in out-of-plane directions with a donut-like shape. The size

of the oscillating medium is less than ~λ/2, estimated from the displacement field demonstrated

in Fig. 2(d), which suggests that the strain, and therefore the output voltage with the same sign

inside the defect, would have a size smaller than λ/2. When the diameter is larger than λ/2, the
piezoelectric ceramic covers the area under strains with opposite signs, and voltage cancellation

takes place.

Output power and output power density of the MEH system with different diameters are also

obtained from calculation using Ohm’s law, as demonstrated in Fig. 2(b). The maximum output

power and output power density at the corresponding power-optimal electrical loading

resistances are replotted as a function of diameters in Fig. 2(c). Here, the noteworthy feature is

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that an optimal diameter of 8 mm exists, which maximizes the output power generation of 1.7

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mW. The open-circuit voltage increases with decreasing diameter, as shown in Fig. 2(a).

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Meanwhile, the power-optimal electrical loading resistances that maximize the power generation
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likewise increase with decreasing diameter, as shown in Fig. 2(b). Thus, the trade-off between
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the voltage cancellation effect at the strain nodes of the PnC and the size dependence of the

power-optimal electrical loading conditions results in the generation of maximum power when
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the diameter is 8 mm. On the other hand, when we incorporate the operating volume factor, the
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smallest diameter of 6 mm offers the highest output power density of 31 mW/cm3. Thus,
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selecting a different diameter of a PEH is necessary depending on target performance metric to

maximize: output power or output power density.

Another geometric factor we considered here is the thickness of the PEH. The output voltage

of a given PEH can be generally expressed by the following equation [39]:

= × × × (1)

where k is the electromechanical coupling factor, g is the piezoelectric voltage constant, t depicts

the thickness of the device, and σ is the mechanical stress applied to the piezoelectric ceramic.
Eq. (1) suggests a linear relationship between the output voltage and thickness of the PEH, in the

case of constant applied stress. The applied stress term, σ, is directly related to the amount of

energy transferred to the PEH from the defect in the PnC supercell. In elastic waves, energy is

transferred through motions of particles in solids [40]. In our system, the incident elastic waves

propagate through a single layer (i.e., an aluminum plate with a PnC supercell) and encounter bi-

layer structures consisting of the aluminum plate and piezoelectric ceramic, as depicted in the

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inset of Fig. 2(e). At the boundary, both reflection and transmission of waves take place. The

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transmitted waves penetrate through the bi-layer structure and provide elastic energy into the

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PEH, whereas reflected waves return to the single aluminum layer and thus do not contribute to
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the harvesting. Thus, the amount of elastic wave energy transferred at the boundary can be
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estimated using the transmission parameter, T, which can be calculated in terms of the ratio of

the mechanical impedance, Zm, of each component layer, as expressed in Eq. (2) [41]:
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= ,
(2)
, ,
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In Eq. (2), Zm,Al denotes the mechanical impedance of the aluminum layer, and Zm,Bi is the

effective mechanical impedance of the bi-layer structure consisting of PnC medium material and

PEH. Derivation of the following Eq. (3) for Zm,Bi in Supplementary S7 indicates that Zm,Bi has a

linear relation with the square of the thickness of the PEH, t:

√ ×
, = × ! × ( + 2) (3)
where ρeff, Eeff, and veff are the effective density, Young’s modulus, and Poisson’s ratio for the bi-

layer structure, respectively. If we insert Eq. (3) into the transmission Eq. (2), the final

expression reveals that the transmitted energy is inversely proportional to the square of PEH

thickness, t, which is the only tunable parameter when the material properties are given. Fig. 2(e)

shows the calculated PEH thickness dependence of transmittance, where it is clearly observed

that the transmission T is likely to decrease as thickness of the PEH increases. Larger PEH

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thickness leads to larger mechanical impedance mismatch, with less energy transmitted to the

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PEH device. To sum up, there would be two competing contributions to the harvesting power

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output in terms of the PEH thickness of the PnC-based EH system: increased voltage generation
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according to Eq. (1) and lower energy transmission with increasing thicknesses as shown in Fig.
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2(e) derived from Eq. (3).

To experimentally verify the two competing effect of the PEH thickness on the overall MEH
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power generation, we fabricated six different PEH devices with various thicknesses ranging from
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0.5 mm to 3.0 mm, while fixing the diameter at 8 mm and maintaining the composition the same
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as 0.23PZ-0.36PT-0.41PNN (specimen #1 in Table 1). Fig. 2(f) shows that increasing the

thickness from 0.5 mm up to 2.5 mm apparently leads to higher open-circuit voltage generation,

followed by the presence of saturated voltage values around 4.6 V when the thickness exceeds

2.0–2.5 mm. The plot of output power versus electrical resistance in Fig. 2(g) is replotted in Fig.

2(h) as a function of thickness, where we can clearly confirm that there is an optimal thickness

between 2.0 mm and 2.5 mm that gives rise to the maximum power generation of 2.3 mW as a

result of two competing mechanisms. Furthermore, taking the operating volume into

consideration results in the thickness of 2.0 mm which enables both output power and output

power density (23 mW/cm3) at their maxima. Therefore, both theoretical and experimental
analysis results support that there is certainly a tradeoff between high voltage generation and

lower energy transfer with increasing thickness. Up to 2-mm thickness, the piezoelectric ceramic

thickness dominates the contribution to voltage and increasing power generation, while for

piezoelectric ceramics thicker than 2 mm, a decrease in the wave energy transmission dominates

the effect of the overall power generation and yields optimal values. Note that the proper

thickness of a PEH suitable for a different PnC based-EH system needs to be determined

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differently if there is any change in either geometric or material properties of either the PnC

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medium layer or PEHs, according to Eq. (3). It is noteworthy that the geometric parameter

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variation of a PEH can effectuate a substantial change in the output power, e.g., ranging from
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0.07 mW to 2.40 mW as shown in Fig. 2(c) and 2(h), even for the same PnC designs. This offers
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tunable capability and design flexibility of PnC-based EH systems by tailoring only the

geometric device designs of PEHs.


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2.3 Enhanced energy conversion through high d × g piezoelectric materials


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Once elastic wave energy is transferred from the PnC to the PEH, efficient conversion from

elastic strain energy to electrical energy via piezoelectric effect becomes crucial for power

generation. As an evaluation criteria for energy conversion in vibration energy harvesting, the

product of the piezoelectric charge coefficient d × g has been known as a figure-of-merit (FOM)

of piezoelectric materials, especially under off-resonance conditions, while the mechanical

quality factor, Qm, and the electromechanical coupling factor, k, also are involved in determining

the FOM near or at resonance conditions [42,43]. However, little is known regarding the

piezoelectric materials selection criteria suitable for the MEH, in particular, the PnC-based EH.

To account for the well-known piezoelectric properties including d × g, k, and Qm, we carefully
selected the composition and constituent materials to achieve the following three groups of

piezoelectric ceramics with a total of eight specimens listed in Table 1. The first group

(specimens #1, #2, #3 in Table 1) belongs to the relaxor PNN-based PZT ternary systems (Fig.

3(a)), which exhibit typical soft-type ceramic characteristics with large piezoelectric charge

coefficients, dielectric coefficients, electromechanical coupling factor, and low mechanical

quality factor [44]. Although compositions of the specimens #1, #2, and #3 all belong to the

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rhombohedral-tetragonal morphotropic phase boundary (R-T MPB) region in the ternary phase

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diagram as illustrated in Fig. 3(a), tailoring the detailed piezoelectric material properties among

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these specimens is possible by composition variation of the relaxor PNN. The resulting material
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properties are listed in Table 1. The second group, specimens #4 and #5 in Table 1, depicts the
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acceptor-doped hard piezoelectric ceramics that are characterized by small piezoelectric charge

coefficients, small values for permittivity, and large mechanical quality factors, relative to soft
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ceramics. We differentiated specimens #4 and #5 by the amount of Mn doping into the relaxor
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PZN-based PZT ternary systems, so as to mainly tune the Qm. For comparison with the lead-
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based ceramics in the first and second groups, the third group consists of three representative

lead-free ceramics with various piezoelectric properties, that is, BaTiO3-based ceramics and

CuO-doped (K,Na)NbO3-based ceramics. Supplementary S8 provides a detailed description of

the working mechanism that gives rise to the resulting piezoelectric, dielectric, and mechanical

properties depending on the relaxor type, composition, and Mn doping. The X-ray diffraction

(XRD) patterns shown in Fig. S10-i and the scanning electron microscopy (SEM) images in Fig.

S10-ii also confirm that all these piezoelectric ceramics are synthesized with dense

microstructures consisting of homogeneous perovskite structures without any secondary phases.

To eliminate the geometric effect on the EH performance, all eight samples are fabricated in the
same geometric dimension of 8-mm diameter and 2-mm thickness, which proved to be the best

geometric values for our given PnC-based EH system.

Higher voltage generation is largely observed in MEH more with lead-based piezoelectric

ceramics than with lead-free piezoelectric ceramics, as shown in Fig. 3(b). This is not always the

case from the perspective of power generation, as shown in Fig. 3(c) and 3(d). For example, the

lead-free specimen #6 demonstrated the capability to generate comparable or even improved

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output power when compared to lead-based specimens #4 and #5. Regardless of whether the

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specimen is lead-based or lead-free, a notable observation can be made, as shown in Fig. 3(d),

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that the rise in the value of d × g leads to an increase in the output power generation of the PnC-
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based MEH system. The specimen #2 (0.32PZ-0.39PT-0.29PNN), which has the largest value of
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d × g, yields the maximum output power of 2.7 mW. Since resonant frequencies of the

piezoelectric disks with the given dimensions are in the range of 232~452 kHz, as tabulated in
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the Supplementary S9, and the excitation frequency is 50 kHz, this implies that all eight disks
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operate under off-resonant conditions. Therefore, the conclusion can be drawn here that the FOM
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of d × g, conventionally used for vibration EH systems at off-resonance, can be adopted in the

PnC-based MEH systems. The trend of power as functions of Qm, as well as d × g, shown in Fig.

3(d) and 3(e), suggests that soft-type ceramics characterized by high d × g and low Qm are more

advantageous for power generation in MEH systems, when compared to the hard-type ceramics,

both in lead-based and lead-free piezoelectric material. The results shown in Fig. 3(e), however,

need to be interpreted carefully. Although power seems to increase with decreasing Qm in Fig.

3(e), this does not mean that low Qm leads to more power generation, since Qm is not the only

influencing factor. Rather, the purpose of this plot is to determine which type of ceramics, i.e.,

soft or hard, are more suitable candidates for enabling enhanced MEH performance. In terms of
the effect of Qm on the power performance, a previous study reported that a small loss in both

mechanical and electrical properties considerably affected the output power generation in

vibration EH systems [45]. Thus, it would be likely that a higher mechanical quality factor,

which is the inverse of mechanical loss, might result in more power generation within the MEH

as well. Therefore, the insight provided by Fig. 3(d) and 3(e) is that the FOM d × g, rather than

Qm, can serve as a dominant factor that governs the overall output power performance, thus

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making soft piezoelectric ceramics more desirable candidates than the hard ones. Evidently, there

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is room for further enhancement by synthesizing soft-type ceramics with improved Qm, which

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can constitute a promising future study, albeit it is beyond our scope regarding this work.
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2.4 Tunable power amplification ratios of PnC-based EH systems

In the MEH system, the degree of power amplification is likewise a particularly important
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performance metric along with the output power and voltage. The amplification ratio refers to the
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ratio of the output power achieved from the PEH device in the presence of metamaterials—PnC
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in this case—to that in the absence of PnC, i.e., in a bare aluminum plate. For example,

amplification by a factor of 25 is obtained for the PEH with the composition of 0.32PZ-0.39PT-

0.29PNN, diameter of 8 mm, and thickness of 2 mm, as it generates maximum power of only

0.11 mW in a bare Al plate, but yields higher maximum power of 2.7 mW—25 times higher—

with a PnC supercell through input wave energy localization, as illustrated in Fig. 4(a). We

investigated how the amplification ratio changes as a function of geometric and material

properties by measuring and comparing the output power performance for each case in the PnC

and the bare plate. Along with the output power variation as shown in the insets, the

corresponding amplification ratios are plotted in Fig. 4(b)-(d) with regard to the diameters,
thicknesses, and material compositions, respectively. Surprisingly, the geometric parameters, i.e.,

both diameter and thickness, cause substantial changes in not only the output power, as indicated

in Fig. (2), but also in the amplification ratio, ranging from 1 to 35, as shown in Fig. 4(b) and

4(c). In contrast, the amplification ratios are less sensitive to the variation in material properties,

ranging from 23.1 to 26.7, as depicted in Fig. 4(d), whereas the output power exhibits a

significant dependence on the material property variations, as shown in Fig. 3. The large

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sensitivity of both the amplification ratio and output power to the geometric parameters in Fig.

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4(b) and 4(c) is attributed to the relatively complicated wave dynamics inside the defect of the

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PnC, which is directly related to the phenomena governed by the wavelength-dependent voltage
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cancellation and mechanical impedance matching. Material properties are relatively independent
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of the wave dynamics, and thus they affect the variation in the amplification ratio both for lead-

based and lead-free ceramics to a lesser degree (Fig. 4(d)). Special emphasis should be placed on
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the fact that the optimal design parameter with respect to the output power does not necessarily
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coincide with the optimal design parameter with respect to the amplification ratio. For example,
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in Fig.4(c), the 2 mm thick PEH device yields the maximum output power, while 1 mm is the

thickness that enables the maximum amplification ratio of 35, among the cases. Therefore,

identification of the proper geometric and material property parameters that suit the target

performance metric is essential at the device design level of a PEH in PnC-based EH system.

Large amplification underpins the drastic enhancement of output power in MEH but does not

always guarantee its maximization of output power.

3. Conclusions
We aim to achieve unprecedented harvesting output power amplification and generation by

tailoring the geometric and material properties of a piezoelectric energy harvesting device that is

integrated into the phononic crystal. Understanding underlying wave physics between a PEH and

a PnC host structure and materials science in piezoelectric ceramics allows to employ the

following three approaches for enhanced energy transfer and conversion: (1) identification of the

proper diameter that avoids voltage cancellation at wavelength-dependent strain nodes, (2)

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identification of the proper thickness that minimizes the mechanical impedance mismatch at the

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interface between the PnC and the EH device and thus promotes transmission of energy for

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conversion and harvesting, and (3) composition-enabled tuning for high d × g value piezoelectric
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materials, particularly soft ceramics that enhances electromechanical conversion efficiency. The
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parametrically tuned PEH device allows realization of drastic enhancement of elastic wave

harvesting power performance of up to 2.7 mW in our PnC-based EH system, which is even


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substantially larger than the output power of 1.6 mW reported in our prior work [23]. We
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envision that this design flexibility in piezoelectric energy harvesting systems can generate
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further synergetic power performance improvement, along with the future development of new

metamaterials concepts integral for further energy localization capability. We expect that this can

be applied to a wide range of self-powered wireless sensing applications, such as in structural

health monitoring for infrastructures, where elastic waves in ultrasonic frequency regimes are

omnipresent.

4. Simulation and Experimental Section

4.1 Computational Modeling and Simulation


A finite element method (COMSOL MULTIPHYSICS version 5.3) is utilized to obtain the

band structure of the designed unit cell. Under the assumption that the PnC supercell with a

defect is periodically arranged, an eigenvalue problem can be formulated by applying periodic

boundary conditions (so-called Floquet–Bloch theorem) to the four edges of the unit cell and to

the governing equations for elastic waves in the PnC supercell. Then, the dispersion curve is

obtained by numerically calculating eigenfrequencies for reciprocal wave vectors in the border

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line of the first irreducible Brillouin zone Γ→X→M→ Γ. Simulation is conducted to analyze

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harmonic wave propagation behavior in the band gap and to investigate the energy localization

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performance in a unidirectional plane wave. The incident flexural wave (Lamb A0 wave) is
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induced by exciting the cross-section of the entire structure in the transverse direction with a
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constant amplitude of 10 nm. To sufficiently excite the plane wave, the distance between the

excitation source and the front of the PnC was set to 150 mm (eight times the wavelength of the
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Lame A0 wave close to 50 kHz). Perfectly matched layers are applied at the boundaries of the
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entire structure as absorbing boundary conditions.


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4.2 Fabrication of Piezoelectric Ceramic Energy Harvesters

Piezoelectric ceramics for PnC-EH systems were fabricated via conventional ceramic

processing. The raw materials used for the lead-based piezoelectric ceramics (specimens #1–5)

are PbO (99.2%, Dansuk Industry, Korea), ZrO2 (99.2%, Z-Tech, USA), TiO2 (99.2%, Sakai

Kagaku, Japan), ZnO (99.2%, Hakusui, Japan), NiO (99.2%, Nikko Rika, Japan), Nb2O5 (99.2%,

Jiujiang, China), and MgO2 (>99.0%, High Purity Chemicals, Saitama, Japan). For the lead-free

piezoelectric ceramics (specimen #6–8), Na2CO3, K2CO3, BaCO3, CaCO3, ZrO2, TiO2, Sb2O5,

and Nb2O5 (> 99.0%, High Purity Chemicals, Saitama, Japan) powders were used. After
weighing, ball-milling was conducted for 24 h to mix the raw materials using zirconia balls and

ethanol in a polypropylene jar. The mixed lead-based powders were dried and calcined at 880 °C

for 4 h. The calcined powders were re-milled in the polypropylene jar using zirconia balls with

the additives. After drying, the lead-based powders were pressed into disks under a pressure of

9.8 MPa (100 kgf cm–2) and sintered at 1150 °C for 2 h. A similar procedure was conducted to

fabricate lead-free piezoelectric ceramics, except for the calcination and sintering temperatures.

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For the 0.50(Ba0.7Ca0.3)TiO3-0.50Ba(Zr0.5Ti0.5)O3 lead-free ceramic (specimen #6), calcination

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and sintering were performed at 1300 °C and 1450 °C for 3h, respectively. The

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0.96(Na0.5K0.5)(Nb0.955Sb0.045)O3-0.04CaTiO3 ceramic with 2.0 mol.% CuO (specimen #7) was
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calcined at 950 °C for 3 h, and then sintered at 960 °C for 6 h. For 1.0 mol.% CuO added
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(Na0.5K0.5)NbO3 ceramic (specimen #8), the calcination and sintering were conducted at 800 °C

for 4 h and 960 °C for 2 h, respectively. Silver was used for the electrode, and it was printed on
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both the top and bottom surfaces of the specimens, as shown in Fig. 1(a-iv); the bottom electrode
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was extended to the top surface for wiring purposes.


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4.3 Characterization of Structural and Material Properties

X-ray diffraction (XRD: D/max-RC; Rigaku, Tokyo, Japan) using CuKα radiation and

scanning electron microscopy (SEM; Hitachi S-4300, Osaka, Japan) were used to investigate

structural and microstructural properties of the ceramics. Piezoelectric ceramics were pooled in

silicone oil at 120 °C by applying a DC field of 3–4 kV mm–1 for 30 min. The piezoelectric and

dielectric properties of specimens were measured using a d33 meter (Piezotest PiezoMeter PM-

100, London, UK) and an impedance analyzer (Agilent Technologies HP 4194A, Santa Clara,

CA, USA) according to IEEE standards.


4.4 Fabrication of PnC-based EH System

The metamaterial, a 5 × 11 supercell PnC structure with a defect, was fabricated by laser

cutting the aluminum plate of 2-mm thickness, as shown in Fig. 1(a-i). A unit cell of the PnC is a

square plate containing an octagon hole, and its size is illustrated in Fig. 1(a-ii). The piezoelectric

ceramic was attached at the center of the defect to harvest the localized wave energy and convert

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it into electrical energy.

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4.5 Characterization of PnC-based EH System Performance
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Piezoelectric transducers (PZT, Ceracomp Co. Ltd.) with a resonant frequency of 50 kHz
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were attached to the aluminum plate to generate elastic waves (A0 Lamb waves). To induce the

plane waves, the distance between the piezoelectric transducer (source) and the PnC must be at
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least 20 times larger than the wavelength of the incident mechanical wave. Tone-burst input
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signals with 20 cycles at 50 kHz were induced from the transducers, which were controlled by
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function generators (Keysight 33512B) and a power amplifier (AE Techron 7224). Mechanical

displacements of the aluminum plate were measured using a laser Doppler vibrometer (Polytec,

PSV-400 and OFV-5000). Further, the elastic wave propagations were visualized via scanning of

the displacements at three different areas; before the PnC, inside the defect of the PnC, and

behind the PnC. The output voltage of the MEH was measured with respect to time and load

resistance, using an oscilloscope (Teledyne LeCroy, Waverunner 610zi). The output power of the

PnC-based EH system was calculated using the output voltage and load resistance using Ohm’s

law. The experimental setup of characterization of the PnC-EH system in this work is shown in

Fig. S6.
Acknowledgments

This research was supported by the National Research Council of Science & Technology

(NST) grant by the Korean government (MSIP; No. CAP-17-04-KRISS). The authors also thank

the KU-KIST Graduate School Program of Korea University.

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List of Table captions

Table 1. Compositions and physical properties of piezoelectric ceramic specimens

List of figure captions

Fig. 1. (a-i) Photograph of fabricated PnC-based EH (PnC-EH) system consisting of 5 × 11 PnC

supercell and a piezoelectric ceramic at defect; (a-ii) Proposed design of a unit cell with

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dimensions and directions; (a-iii) Schematic illustration of elastic wave localization at defect,

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relative to the incident wave; (a-iv) Piezoelectric ceramic with electrode configurations. (b) Band
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structure of designed unit cell, with dispersion relation of frequencies with respect to wave
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number. Band gap is colored in light blue. Formation of seven defects bands at 47.4, 48.8, 49.1,
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50.0, 50.2, 51.2, 51.8 kHz are indicated inside the band gap as solid lines in black. (c) Simulation

of harmonic wave propagation behavior in PnC at 50 kHz. (d) Experimental visualization of


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elastic wave propagation inside defect area. (e) Measured out-of-plane mechanical displacements
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of metamaterial at center of defect of PnC plate and of bare aluminum plate. Variations of (f)
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Output voltage and (g) Output power of PnC-EH system with respect to time and load resistance.

Fig. 2. Variation of (a) Output voltage and (b) Output power with respect to load resistance for

PnC-EH systems with various diameters of piezoelectric ceramic. (c) Variation of output power

and output power density as function of ceramic diameter. (d) Measured elastic wave

propagation before PnC showing incident wave characteristics. Inset shows magnitude of

wavelength of incident elastic waves. (e) Plots of transmission, T, and mechanical impedance of

the bi-layer, Zm,Bi, as a function of ceramic thickness. Inset schematically illustrates cross-section

of PnC-EH system to illustrate boundary between aluminum plate (PnC medium material) and
PEH. Variation of (f) Output voltage and (g) Output power with respect to load resistance for

PnC-EH systems at various thicknesses of ceramic. (h) Variation of output power and output

power density as a function of ceramic thickness.

Fig. 3. (a) Phase diagram of PZ-PT-PNN ternary system where compositions for specimens #1,

#2, and #3 are indicated. Variation of (b) Output voltage and (c) Output power as a function of

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load resistance for PnC-EH systems with piezoelectric ceramics of various compositions. (d)

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Variation of output power of PnC-EH systems with respect to d × g values of i) PZT-based and ii)

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Lead-free piezoelectric ceramics. (e) Variation of output power with respect to Qm values of i)
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PZT-based and ii) Lead-free piezoelectric ceramics.
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Fig. 4. (a) Variation of output power with respect to load resistance for PnC-EH and PEH in bare
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Al plate (Bare-EH), show power amplification by approximately 25 times, attributed to energy


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localization effect of metamaterial; here: PnC. Inset shows variations of output voltage with
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respect to load resistance for both cases, resulting in 4.8-factor enhancement. (b,c) Variation of

power amplification ratio with respect to diameter and thicknesses of PEH devices, respectively.

Insets of Figs. 4(b) and 4(c) show variations of output power for PnC-EH and Bare-EH with

respect to diameter and thickness, respectively. (d) Power amplification ratios of PEH devices

with piezoelectric ceramics of various compositions.


Table 1. Compositions and physical properties of piezoelectric ceramic specimens

Specimen
Compositions d33 [pC∙N–1] g33 [10-3V∙m∙N–1] d33×g33 [10-15 m2∙N–1] εT33/ε0 keff Qm
Number

0.23PbZrO3-0.36PbTiO3-0.41Pb(Ni1/3Nb2/3)O3
#1 820 22.8 18800 4040 0.60 40
[0.23PZ-0.36PT-0.41PNN]

0.32PbZrO3-0.39PbTiO3-0.29Pb(Ni1/3Nb2/3)O3
#2 740 32.5 24000 2580 0.612 50
[0.32PZ-0.39PT-0.29PNN]

0.34PbZrO3-0.40PbTiO3-0.26Pb(Ni1/3Nb2/3)O3
Lead- #3 630 34.1 21300 2070 0.609 60

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[0.34PZ-0.40PT-0.26PNN]
Based
0.35PbZrO3-0.35PbTiO3-0.30Pb(Zn1/3Nb2/3)O3

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Ceramic
#4 + 0.5 mol.% MnO2 420 36.5 15000 1270 0.524 125

[0.35PZ-0.35PT-0.30PZN+0.5%Mn]

0.35PbZrO3-0.35PbTiO3-0.30Pb(Zn1/3Nb2/3)O3
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#5 + 5.0 mol.% MnO2 190 40 7400 520 0.416 250
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[0.35PZ-0.35PT-0.30PZN+5.0%Mn]

0.50(Ba0.7Ca0.3)TiO3-0.50Ba(Zr0.5Ti0.5)O3
#6 540 21.3 11500 2970 0.435 100
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[0.5BCT-0.5BZT]

0.96(Na0.5K0.5)(Nb0.955Sb0.045)O3-0.04CaTiO3
Lead-
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#7 + 2.0 mol.% CuO 220 23 5000 1100 0.394 250


Free
[CNKNS-0.04CT]
Ceramic
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(Na0.5K0.5)NbO3

#8 + 1.0 mol.% CuO 70 30 2100 260 0.248 550

[CNKN]

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Fig. 1. (a-i) Photograph of fabricated PnC-based EH (PnC-EH) system consisting of 5 × 11 PnC

supercell and a piezoelectric ceramic at defect; (a-ii) Proposed design of a unit cell with

dimensions and directions; (a-iii) Schematic illustration of elastic wave localization at defect,

relative to the incident wave; (a-iv) Piezoelectric ceramic with electrode configurations. (b) Band

structure of designed unit cell, with dispersion relation of frequencies with respect to wave
31
number. Band gap is colored in light blue. Formation of seven defects bands at 47.4, 48.8, 49.1,

50.0, 50.2, 51.2, 51.8 kHz are indicated inside the band gap as solid lines in black. (c) Simulation

of harmonic wave propagation behavior in PnC at 50 kHz. (d) Experimental visualization of

elastic wave propagation inside defect area. (e) Measured out-of-plane mechanical displacements

of metamaterial at center of defect of PnC plate and of bare aluminum plate. Variations of (f)

Output voltage and (g) Output power of PnC-EH system with respect to time and load resistance.

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32
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Fig. 2. Variation of (a) Output voltage and (b) Output power with respect to load resistance for
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PnC-EH systems with various diameters of piezoelectric ceramic. (c) Variation of output power
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and output power density as function of ceramic diameter. (d) Measured elastic wave

propagation before PnC showing incident wave characteristics. Inset shows magnitude of

wavelength of incident elastic waves. (e) Plots of transmission, T, and mechanical impedance of

the bi-layer, Zm,Bi, as a function of ceramic thickness. Inset schematically illustrates cross-section

of PnC-EH system to illustrate boundary between aluminum plate (PnC medium material) and

PEH. Variation of (f) Output voltage and (g) Output power with respect to load resistance for

PnC-EH systems at various thicknesses of ceramic. (h) Variation of output power and output

power density as a function of ceramic thickness.


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Fig. 3. (a) Phase diagram of PZ-PT-PNN ternary system where compositions for specimens #1, #2, and #3 are indicated. Variation

of (b) Output voltage and (c) Output power as a function of load resistance for PnC-EH systems with piezoelectric ceramics of

various compositions. (d) Variation of output power of PnC-EH systems with respect to d × g values of i) PZT-based and ii) Lead-

free piezoelectric ceramics. (e) Variation of output power with respect to Qm values of i) PZT-based and ii) Lead-free piezoelectric

ceramics.

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Fig. 4. (a) Variation of output power with respect to load resistance for PnC-EH and PEH in bare Al
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plate (Bare-EH), show power amplification by approximately 25 times, attributed to energy

localization effect of metamaterial; here: PnC. Inset shows variations of output voltage with respect
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to load resistance for both cases, resulting in 4.8-factor enhancement. (b,c) Variation of power
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amplification ratio with respect to diameter and thicknesses of PEH devices, respectively. Insets of

Fig. 4(b) and 4(c) show variations of output power for PnC-EH and Bare-EH with respect to

diameter and thickness, respectively. (d) Power amplification ratios of PEH devices with

piezoelectric ceramics of various compositions.

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Fundamental understanding of the wave energy transfer and conversion at the

interface between the piezoelectric energy harvesting (PEH) devices and the

phononic crystal (PnC), enables identification of proper geometric parameters and

materials figure-of-merit of PEH devices for power enhancement.

Drastic enhancement of elastic wave harvesting power performance of up to 2.7 mW

in our phononic crystal-based energy harvesting system is realized via a parametric

tailored piezoelectric energy harvesting device.

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Tae- Gon Lee received the Ph.D. degree from the Korea University, Seoul, Korea, in 2020.
Currently, he is a staff engineer in the Samsung Electronics. His research interest includes

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piezoelectric ceramics, energy harvesters based on the piezoelectric materials and piezoelectric
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thin film, VNAND flash memory, next-generation memory.
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Soo-Ho Jo is currently pursuing the Ph.D. degree in Mechanical and Aerospace Engineering,
Seoul National University, Seoul, Republic of Korea. He received the B.S. degree from Seoul
National University, Seoul, Republic of Korea, in 2016. His current research topics include
piezoelectric vibration energy harvesting and elastic metamaterials. He was the recipient of the
Bronze Prize from the KSME-SEMES Open Innovation Challenge in 2016, the Best Paper
Award from the KSME in 2018 and 2020, the 2nd Place Winner in the Student Paper
Competition of the KSME in 2018, the Best Paper Award from the KSNVE in 2019, and the 2nd
Place Winner in the PHM Society Data Challenge Competition in 2019.
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Hong Min Seung is a senior research scientist at Korea Research Institute of Standards and

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Science (KRISS). He received his Ph. D degree (2016) in Mechanical Engineering from Seoul
National University, South Korea. His research interests are ultrasonic nondestructive evaluation,
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electromagnetic acoustic transducers (EMATs) and acoustic/elastic metamaterials.
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Sun-Woo Kim received the B.S. degree from the Korea University, Seoul, Korea, in 2017.
Currently he is in the integrated M.S. & Ph.D. course in Korea University. His research interest
includes energy harvesters based on the piezoelectric materials and lead-free piezoelectric
ceramics for actuators.
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Eun-Ji Kim is currently in the integrated M.S. & Ph.D. course in Korea University, Seoul,

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Republic of Korea. Her current research interests include vibration energy harvesters and
actuators based on the piezoelectric materials. She was the recipient of Paper Award from the
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Materials Research Society of Korea (2016, 2017).
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Byeng D. Youn is the Full Professor of Mechanical and Aerospace Engineering at Seoul
National University (SNU) and the founder and CEO of OnePredict Inc. (onepredict.com). Prof.
Youn received the B.S. degree in mechanical engineering from Inha University, Incheon, South
Korea, in 1996, the M.S. degree in mechanical engineering from Korea Advanced Institute of
Science & Technology, Daejeon, South Korea, in 1998, and the Ph.D. degree in mechanical
engineering from the University of Iowa, Iowa City, IA, USA, in 2001. His current research
includes prognostics and health management (PHM), engineering design under uncertainty, and
energy harvester design. His dedication and efforts in research have garnered substantive peer
recognition resulting in many notable awards including the Commendation of Prime Minister
(2019), the Shin Yang Academic Award from Seoul National University (2017), the IEEE PHM
Competition Winner (2014), the PHM Society Data Challenge Winners (2014, 2015, 2017,
2019), etc.
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Sahn Nahm received the Ph.D. degree from University of Maryland, College Park, in 1990. And

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he was a Postdoctoral course Research Associate with the University of Maryland between 1991
and 1992. He was a Senior Researcher in the Electronic Telecommunication Research Institute
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from 1992 to 1995 and moved to Keimyung University, Dae-gu, Korea, in 1995. Since February
1996, has been with the faculty of the Department of Materials Science and Engineering, Korea
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University, where he is a Professor and the Head of the Electro-Ceramics Laboratory. His
research fields are the dielectric thin films, piezoelectric ceramics, ZnS, and ReRAM.
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Miso Kim is a senior research scientist at Korea Research Institute of Standards and Science
(KRISS). She received her undergraduate degree in Materials Science and Engineering from
Seoul National University, South Korea (2004). She received her M.S. (2007) and Ph.D. degrees
(2012) in Materials Science and Engineering from the Massachusetts Institute of Technology
(MIT). She joined the Center for Safety Measurement of KRISS as a senior research scientist in
2012 and has happily pursued her passion for research at KRISS since then. Her primary
research interests cover analytical modeling, design, and experimental characterization of
piezoelectric materials and smart structures (including mechanical metamaterials) for energy
harvesting and sensing.

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Declaration of interests

☒ The authors declare that they have no known competing financial interests or personal relationships
that could have appeared to influence the work reported in this paper.

☐The authors declare the following financial interests/personal relationships which may be considered
as potential competing interests:

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